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At least 649 records · Page 36

RXTE Observations of LMC X-1 and LMC X-3

Of all known persistent stellar-mass black hole candidates, only LMC X-1 and LMC X-3 consistently show spectra that are dominated by a soft, thermal component. We present results from long (170 ksec) Rossi X-ray Timing Explorer (RXTE) observations of LMC X-1 and LMC X-3 made in 1996 December. The spectra can be described by a multicolor disk blackbody plus an additional high-energy power-law. Even though the spectra are very soft (Gamma approximately 2.5), RXTE detected a significant signal from LMC X-3 up to energies of 50 keV, the hardest energy at which the object was ever detected. Focusing on LMC X-3, we present results from the first year of an ongoing monitoring campaign with RXTE which started in 1997 January. We show that the appearance of the object changes considerably over its approximately 200d long cycle. This variability can either be explained by periodic changes in the mass transfer rate or by a precessing accretion disk analogous to Her X-1.

Wilms, J.↗

RXTE Observations of LMC X-1 and LMC X-3

Of all known persistent stellar-mass black hole candidates, only LMC X-1 and LMC X-3 consistently show spectra that are dominated by a soft, thermal component. We present results from long (170 ksec) Rossi X-ray Timing Explorer (RXTE) observations of LMC X-1 and LMC X-3 made in 1996 December. The spectra can be described by a multicolor disk blackbody plus an additional high-energy power-law. Even though the spectra are very soft (Gamma approximately 2.5), RXTE detected a significant signal from LMC X-3 up to energies of 50 keV, the hardest energy at which the object was ever detected. Focusing on LMC X-3 , we present results from the first year of an ongoing monitoring campaign with RXTE which started in 1997 January. We show that the appearance of the object changes considerably over its approximately 200 d long cycle. This variability can either be explained by periodic changes in the mass transfer rate or by a precessing accretion disk analogous to Her X-1.

Wilms, J.↗

[Presentation Slides] Code-to-Code Benchmark Study for Thermal Stress Modeling and Preliminary Analysis of the High-temperature Single Heat-Pipe Experiment

In the heat-pipe-cooled microreactor, heat pipes remove heat from the reactor core as a passive heat-transfer device, so the fluid circulation is not required for cooling, which can substantially simplify the overall reactor design. However, given the extremely high temperatures in the core region and potentially large temperature gradients across the structure materials, thermal stresses need to be well-analyzed to ensure structural integrity during normal operations and accident scenarios. This presentation slides discuss finite element method-based thermal-stress analysis for the high-temperature single heat-pipe test article in the Single Primary Heat Extraction and Removal Emulator (SPHERE) facility at Idaho National Laboratory (INL), using two commercial software packages, Abaqus and Star-CCM+. A code-to-code benchmark study was performed to crosscheck the model setup and capability of each code and to gain preliminary insights into the potential thermal stress concerns from the current experimental setup. It is observed the significant thermal stresses happen at the inner surface of the heat pipe hole surrounded by electric heaters where the largest temperature gradients appear. The temperature fields have good agreements between Abaqus and Star-CCM+, while the induced thermal stresses show modest deviations probably due to differences of meshing engines used in these two codes. It is found that the local maximum thermal stresses may reach close to the ultimate tensile strength and yield strength of structural material depending on the heater power. Ultimately, the coupled thermal-structural analysis will help guide the current experimental plan and ensure the facility safety for future experimental study.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Photoexcitation of Fe 3 O Nodes in MOF Drives Water Oxidation at pH=1 When Ru Catalyst Is Present

Abstract Artificial photosynthesis strives to convert the energy of sunlight into sustainable, eco‐friendly solar fuels. However, systems with light‐driven water oxidation reaction (WOR) at pH=1 are rare. Broadly used [Ru(bpy) 3 ] 2+ (bpy=2,2’‐bipyridine) photosensitizer has a fixed +1.23 V potential which is insufficient to drive most water oxidation catalysts (WOCs) in acid, while Fe 2 O 3 , featuring the highly oxidizing holes, is not stable at low pH. Here, the key examples of Fe‐based metal–organic framework (MOF) water oxidation photoelectrocatalysts active at pH=1 are presented. Fe‐MIL‐126 and Fe MOF‐dcbpy structures were formed with 4,4’‐biphenyl dicarboxylate (bpdc), 2,2’‐bipyridine‐5,5’‐dicarboxylate (dcbpy) linkers and their mixtures. Presence of dcbpy linkers allows integration of metal‐based catalysts via coordination to 2,2’‐bipyridine fragments. Fe‐based MOFs were doped with Ru‐based precursors to achieve highly active MOFs bearing [Ru(bpy)(dcbpy)(H 2 O) 2 ] 2+ WOC. Materials were analyzed with X‐ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infra‐red (FTIR) spectroscopy, resonance Raman, X‐ray absorption spectroscopy, fs optical pump‐probe, electron paramagnetic resonance (EPR), diffuse reflectance and electric conductivity measurements and were modeled by band structure calculations. It is shown that under reaction conditions, Fe III and Ru III oxidation states are present, indicating rate‐limiting electron transfer in MOF. Fe 3 O nodes emerge as photosensitizers able to drive prolonged O 2 evolution in acid. Further developments are possible via MOF's linker modification for enhanced light absorption, electrical conductivity, reduced MOF solubility in acid, Ru‐WOC modification for faster WOC catalysis, or Ru‐WOC substitution to 3d metal‐based systems. The findings give further insight for development of light‐driven water splitting systems based on Earth‐abundant metals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Semiautomated, Reproducible Batch Processing of Soy

A computer-controlled apparatus processes batches of soybeans into one or more of a variety of food products, under conditions that can be chosen by the user and reproduced from batch to batch. Examples of products include soy milk, tofu, okara (an insoluble protein and fiber byproduct of soy milk), and whey. Most processing steps take place without intervention by the user. This apparatus was developed for use in research on processing of soy. It is also a prototype of other soy-processing apparatuses for research, industrial, and home use. Prior soy-processing equipment includes household devices that automatically produce soy milk but do not automatically produce tofu. The designs of prior soy-processing equipment require users to manually transfer intermediate solid soy products and to press them manually and, hence, under conditions that are not consistent from batch to batch. Prior designs do not afford choices of processing conditions: Users cannot use previously developed soy-processing equipment to investigate the effects of variations of techniques used to produce soy milk (e.g., cold grinding, hot grinding, and pre-cook blanching) and of such process parameters as cooking times and temperatures, grinding times, soaking times and temperatures, rinsing conditions, and sizes of particles generated by grinding. In contrast, the present apparatus is amenable to such investigations. The apparatus (see figure) includes a processing tank and a jacketed holding or coagulation tank. The processing tank can be capped by either of two different heads and can contain either of two different insertable mesh baskets. The first head includes a grinding blade and heating elements. The second head includes an automated press piston. One mesh basket, designated the okara basket, has oblong holes with a size equivalent to about 40 mesh [40 openings per inch (.16 openings per centimeter)]. The second mesh basket, designated the tofu basket, has holes of 70 mesh [70 openings per inch (.28 openings per centimeter)] and is used in conjunction with the press-piston head. Supporting equipment includes a soy-milk heat exchanger for maintaining selected coagulation temperatures, a filter system for separating okara from other particulate matter and from soy milk, two pumps, and various thermocouples, flowmeters, level indicators, pressure sensors, valves, tubes, and sample ports

Thoerne, Mary↗

Salt Vessel-Sample Generator Interface

The goal of the salt sampling program at Argonne is to develop and deploy automated molten salt sampling approaches for interfacing relevant unit operations with salt analysis to improve the timeliness and accuracy of sampling-based accountancy measurements. One technology under development is a vacuum sampler loop module. In this system, molten salt is drawn from a process vessel through a heated sampling line and into a charge vessel. Next, one or more samples are split from the volume in the charge vessel and the remaining salt is returned to the process. The vacuum sampler loop module is being developed to interface with other sample processing and analysis modules to enable rapid at-line sample characterization. The main purpose of the vacuum sampling loop module is to enable the collection of samples that are more representative of the bulk salt by replacing traditional point samplers (i.e., dip probes) with a sampling approach that captures a larger cross section of salt. Additionally, the vacuum sampling approach eliminates the risk of dross contamination of samples and avoids the use of moving parts in the salt. Two methods of interfacing the vacuum sampling loop with a precision pneumatic sample generator were investigated in FY21. This report covers the testing of fluidic coupling between the two modules. Two iterations of the fluidically coupled modules were tested. The first iteration system coupled the two modules using a freeze valve to seal the vacuum sampler during filling and to control flow into the pneumatic sample generator. While this integrated system functioned as intended, some changes were implemented to make the system more robust and better suited to remote deployment. Specifically, the system was made to be more modular and active control of the vacuum filling operation was replaced with a passive control mechanism. For passive filling, the salt charge vessel was vented to a small gas tank that was at negative pressure, causing salt to be drawn into the vessel until the force of the fluid head was in equilibrium with the gas pressure. The passive control system performed well and will be used in future iterations. Another change in the second system was a newly configured pneumatic sample generator in which sample ejection occurred through a hole in the reservoir’s stainless-steel side wall instead of through a non-wetted sapphire orifice on the bottom. This alternate configuration may be better suited for near-process deployment because it enables on-line orifice maintenance and an orifice bypass drain back to the process. A third change in the second iteration system was the transition to a two-chamber charge vessel which split off a fraction of the sampled salt as a liquid aliquot. The goal was to create a buffer mechanism that would allow reproducible aliquoting of samples, independently of variability in the charge vessel fill height. While the two-chamber design was functional, the sample size reproducibility was below target values. To improve reproducibility and overcome many of the impediments to remote deployment of the vacuum sampling loop module, separate work was conducted to replace the two-chamber liquid aliquoting mechanism with aliquoting into single-use sample tubes. Solid salt transfer in the sample tubes will replace fluidic coupling for integrating the vacuum sampler with downstream modules. Because the proposed operations can all be executed with simple overhead actuation mechanisms or other existing hot-cell technology, there will be no need for large investments in novel hot cell sample handling technologies using this alternate approach. As such, near-term deployment of the vacuum sampling technology will be achievable. This new approach for automated coupling of sample tubes with down-stream modules is covered in a separate FY21 report, and a remotely operated version of the vacuum sampler loop module with the tube aliquoting feature is planned for FY22.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Plasmonic Ag nanocomposite phosphate glasses produced via γ-ray irradiation as reduction route

This paper reports on the impact of γ-ray irradiation (10, 100 kGy) on melt-quenched Ag + -doped phosphate glass and the effects of subsequent thermal processing leading to the production of plasmonic Ag nanocomposites. The γ-irradiated glasses were characterized alongside the pristine by differential scanning calorimetry (DSC), Raman spectroscopy, electron paramagnetic resonance (EPR) spectroscopy, optical absorption, and photoluminescence (PL) spectroscopy. DSC characterization showed consistent glass transition temperatures (T g ) before and after γ-irradiation whereas the crystallization temperatures tended to decrease with increasing γ-ray dose. However, a lack of alteration of the glass network structure was supported by Raman spectroscopy. Room temperature EPR spectra clearly showed the formation of phosphorus oxygen hole center (POHC) defects in the undoped host, in addition to another doublet likely associated with a P 3 defect. The presence of paramagnetic silver species encompassing Ag 2+ and 107/109 Ag 0 atoms was also indicated in the silver-activated glass together with POHC defects. Optical absorption spectra were also consistent with the presence of various radiation-induced centers. Further analyzing the glass absorption edge via Tauc plots suggested the formation of electron center (EC) defects in γ-irradiated samples wherein the silver-doped glass exhibited decreasing band gap energies with increasing γ-ray dose. The PL characterization showed the silver-related radio-PL effect was induced exhibiting broad band emission with two maxima around 500 and 625 nm stemming from various molecular Ag$^{x+}_{n}$ clusters. Emission decay analyses revealed that the longer wavelength emission exhibited slower decay. The highest radiation dose of 100 kGy however resulted in weaker emission and faster decay kinetics attributed to energy transfer between the luminescent silver species and POHC defects. Finally subjecting the γ-irradiated Ag-doped glasses to heat treatment near the T g at 490 °C led to the development of the surface plasmon resonance of Ag nanoparticles (NPs) and the vanishing of the Ag$^{x+}_{n}$ clusters luminescence. In conclusion, the presence of the matrix-related EC defects was deemed accountable for the thermally induced reduction and consequent precipitation of Ag NPs making the plasmonic glasses attractive for photonic applications such as nonlinear optics.

36 MATERIALS SCIENCE↗

Boride-Carbon Hybrid Technology to Produce Ultra-Wear and Corrosion Resistant Surfaces for Applications in Harsh Conditions (Final Technical Report)

Engineered functional surfaces play an important role to enable new products and manufacturing processes that can endure harsh service conditions such as high impact and contact loads, highly abrasive wear, extreme temperatures, and corrosive environments. Engineered surfaces can also be instrumental to improving the efficient use of energy by reducing frictional losses and extending service life. The main objective of this project was to develop a hybrid surface engineering technology that combines the advantages of a novel ultrafast boriding process with the next generation of superhard carbon coatings. The hypothesis was that this hybrid process will offer an unprecedented combination of wear and corrosion resistance, low frictional losses and affordability for treated parts so that it can be utilized in many applications. During this project, a duplex process was developed that combines the advantages of ultra-fast electrochemical boriding with those of hard tetrahedral amorphous carbon coatings. Both technologies can be combined to form a hybrid technology that is characterized by low friction and wear properties combined with corrosion and fatigue resistance. Good adhesion of both layers to each other was one main goal of this project, that has been achieved with HF1 adhesion through the Rockwell-C adhesion test. In this project, the mechanical properties of the hybrid coating were modeled through a finite-element analysis approach. We can conclude that the FEA model resembles the actual samples and be utilized to predict mechanical behavior under impacts. Based on this model, application-oriented load conditions can be simulated for optimal layer design regarding thickness and mechanical properties. To exemplify, one conclusion that can be drawn from the nanoindentation model is a boride layer thickness of 50 µm is sufficient to effectively support the carbon coating on the identified AISI 1045 low carbon steel substrate material. The duplex treatment yields wear rates as low as 6 x 10 -8 mm 3 N -1 m -1 and a coefficient of friction of 0.14 when tested against a steel counter face in a ball-on-disk test setup. On the other hand, the wear rate of the only-borided AISI 1045 steel was 5 x 10 -5 mm 3 N -1 m -1 , about three orders of magnitude higher than the duplex coating. At the same time, duplex treated samples experience corrosion resistance, which could not be achieved with single-layer carbon coatings. The developed surface treatment withstands a 3-hour exposure to 15% HCl, while the only carbon coated counter sample shows severe delamination of the coating due to pin hole corrosion. The boride layer is chemically stable and pin hole free because it is formed through an electrochemical process under high current densities (700 mA/cm 2 ) and high temperature. Additionally, the hybrid coating led to at least 3x increase in fatigue strength of the steel substrate, which exceeds the target performance of 30% improvement. There are numerous potential applications for the duplex coatings. A representative application is bearing ball coatings for off-shore windmills. Compared to currently employed surface technologies in this field, the initial costs of applying our technology might be higher due to more process steps but the performance benefits lead to an increased life time of treated parts, which will lower the maintenance and replacement costs in the long-term. To validate the technology for this specific application, the team is currently investigating the process of white etching crack initiation of the duplex coating in collaboration with ANL. Overall, this project successfully validated that the boride-carbon hybrid technology can withstand harsh conditions. One possible approach to commercialization under consideration is to transfer the technology to a startup or an existing coatings company.

36 MATERIALS SCIENCE↗

Facets control charge separation during photoelectrochemical water oxidation with strontium titanate (SrTiO 3 ) single crystals

The photocatalytic overall water splitting reaction provides a pathway to hydrogen fuel from sunlight. Photocatalysts must achieve the reaction without the application of an external bias, which requires an effective charge separation mechanism. Photolabeling studies and electrostatic simulations for the well-known CoOOH/Al:SrTiO 3 /Rh/Cr 2 O 3 photocatalyst suggest that charge separation is driven by work function differences at the (100) and (110) facets of SrTiO 3 , which are electron and hole selective, respectively. Here we use hydrogen annealed SrTiO 3–x single crystals to obtain the first quantitative assessment of the charge separation ability of the (100), or (110), or (111) facets during oxygen evolution. Under UV illumination (60 mW cm –2 ), the crystals exhibit variable water oxidation photocurrents (0.34, 0.82, 1.36 mA cm –2 at 1.23 V versus RHE) and photovoltage values of 1.40, 1.52 and 1.52 V for (100), (110), and (111) SrTiO 3–x , respectively. A surface photovoltage increase in that same order (0.31 V < 0.57 V < 0.67 V) is confirmed independently with vibrating Kelvin probe surface photovoltage spectroscopy (VKP-SPV) under 375 nm (1.91 mW cm –2 ) illumination. Mott Schottky measurements in aqueous K 3/4 [Fe(CN) 6 ] reveal facet-dependent flatband positions of –0.58, –0.71, and –0.74 V RHE for the (100), (110), and (111) crystals respectively. This confirms that the photoelectrochemical water oxidation performance of SrTiO 3–x crystals is controlled by the work function of each facet, which determines the electron transfer barrier height of the respective solid–liquid junctions. After correcting for differences in electron donor concentrations, barriers are found to increase in the order (100) < (111) < (110) and differ by as much as 0.16 eV, similar to an earlier prediction. Altogehter, these results explain the charge separation mechanism in SrTiO 3 photocatalysts and highlight the need for faceted semiconductor crystals as light absorbers in particle-based photocatalysts.

08 HYDROGEN↗

On Alfvénic turbulence of solar wind streams observed by Solar Orbiter during March 2022 perihelion and their source regions

It has been recently accepted that the standard classification of the solar wind solely according to flow speed is outdated, and particular interest has been devoted to the study of the origin and evolution of so-called Alfvénic slow solar wind streams and to what extent such streams resemble or differ from fast wind. In March 2022, Solar Orbiter completed its first nominal phase perihelion passage. During this interval, it observed several Alfvénic streams, allowing for characterization of fluctuations in three slow wind intervals (AS1-AS3) and comparison with a fast wind stream (F) at almost the same heliocentric distance. This work makes use of Solar Orbiter plasma parameters from the Solar Wind Analyzer (SWA) and magnetic field measurements from the magnetometer (MAG). The magnetic connectivity to the solar sources of selected solar wind intervals was reconstructed using a ballistic extrapolation based on measured solar wind speed down to the (spherical) source surface at 2.5 R s below which a potential field extrapolation was used to map back to the Sun. The source regions were identified using SDO/AIA observations. A spectral analysis of in situ measured magnetic field and velocity fluctuations was performed to characterize correlations, Alfvénicity, normalized cross-helicity, and residual energy in the frequency domain as well as intermittency of the fluctuations and spectral energy transfer rate estimated via mixed third-order moments. A machine learning technique was used to separate proton core, proton beam, and alpha particles and to study v − b correlations for the different ion populations in order to evaluate the role played by each population in determining the Alfvénic content of solar wind fluctuations. The comparison between fast wind and Alfvénic slow wind intervals highlights the differences between the two solar wind regimes: The fast wind is characterized by larger amplitude fluctuations, and magnetic and velocity fluctuations are closer to equipartition of energy. In fact the Alfvénic slow wind streams appear to be on a spectrum of wind types, with AS1, originating from open field lines neighboring active regions and displaying similarities with the fast wind in terms of fluctuation amplitude and turbulence characteristics, but not with respect to the alpha particles and proton beams. The other two slow streams differed both in their sources as well as plasma characteristics, with AS2 coming from the expansion of a narrow coronal hole corridor and AS3 from a region straddling a pseudostreamer. The latter displayed the coldest and highest density but the slowest stream with the smallest fluctuation amplitude and greatest magnetic energy excess. It also showed the largest scatter in proton beam speeds and the greatest difference in speed between proton beam and alpha particles. This study shows how the old fast–slow solar wind dichotomy, already called into question by the observations of slower Alfvénic solar wind streams, should further be refined, as the Alfvénic slow wind, originating in different solar wind regions, show significant differences in density, temperature, and proton and alpha-particle properties in the inner heliosphere. The observations presented here provide the starting point for a better understanding of the origin and evolution of different solar wind streams as well as the evolving turbulence contained within.

magnetohydrodynamics (MHD)↗

Trap States in Reduced Colloidal Titanium Dioxide Nanoparticles Have Different Proton Stoichiometries

Added electrons and holes in semiconducting (nano)materials typically occupy “trap states,” which often determine their photophysical properties and chemical reactivity. However, trap states are usually ill-defined, with few insights into their stoichiometry or structure. Our laboratory previously reported that aqueous colloidal TiO 2 nanoparticles prepared from TiCl 4 + H 2 O have two classes of electron trap states, termed Blue and Red. Herein, we show that the formation of Red from oxidized TiO 2 requires 1e – + 1H + , while Blue requires 1e – + 2H + . The two states are in a protic equilibrium, Blue ⇌ Red + H + , with K eq = 2.65 mM. The Blue states in the TiO 2 NPs behave just like a soluble molecular acid with this K eq as their K a , as supported by solvent isotope studies. Because the trap states have different compositions, their population and depopulation occur with the making and breaking of chemical bonds and not (as commonly assumed) just by the movement of electrons. In addition, the direct observation of a 2H + /1e – trap state contradicts the emerging H atom transfer (1H + /1e – ) paradigm for oxide/solution interfaces. Finally, this work emphasizes the importance of chemical stoichiometries, not just electronic energies, in understanding and directing the reactivity at solid/solution interfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

On the Star Formation-AGN Connection at zeta (is) approximately greater than 0.3

Using the spectra of a sample of approximately 28,000 nearby obscured active galaxies from Data Release 7 of the Sloan Digital Sky Survey (SDSS), we probe the connection between active galactic nucleus (AGN) activity and star formation over a range of radial scales in the host galaxy. We use the extinction-corrected luminosity of the [O iii] 5007A line as a proxy of intrinsic AGN power and supermassive black hole (SMBH) accretion rate. The star formation rates (SFRs) are taken from the MPA-JHU value-added catalog and are measured through the 3 inch SDSS aperture. We construct matched samples of galaxies covering a range in redshifts. With increasing redshift, the projected aperture size encompasses increasing amounts of the host galaxy. This allows us to trace the radial distribution of star formation as a function of AGN luminosity. We find that the star formation becomes more centrally concentrated with increasing AGN luminosity and Eddington ratio. This implies that such circumnuclear star formation is associated with AGN activity, and that it increasingly dominates over omnipresent disk star formation at higher AGN luminosities, placing critical constraints on theoretical models that link host galaxy star formation and SMBH fueling. We parameterize this relationship and find that the star formation on radial scales (is) less than 1.7 kpc, when including a constant disk component, has a sub-linear dependence on SMBH accretion rate: SFR in proportion to solar mass(sup 0.36), suggesting that angular momentum transfer through the disk limits accretion efficiency rather than the supply from stellar mass loss.

LaMassa, Stephanie M.↗

Boundary Layer Control for Hypersonic Airbreathing Vehicles

Active and passive methods for tripping hypersonic boundary layers have been examined in NASA Langley Research Center wind tunnels using a Hyper-X model. This investigation assessed several concepts for forcing transition, including passive discrete roughness elements and active mass addition (or blowing), in the 20-Inch Mach 6 Air and the 31-Inch Mach 10 Air Tunnels. Heat transfer distributions obtained via phosphor thermography, shock system details, and surface streamline patterns were measured on a 0.333-scale model of the Hyper-X forebody. The comparisons between the active and passive methods for boundary layer control were conducted at test conditions that nearly match the Hyper-X nominal Mach 7 flight test-point of an angle-of-attack of 2-deg and length Reynolds number of 5.6 million. For passive roughness, the primary parametric variation was a range of trip heights within the calculated boundary layer thickness for several trip concepts. The passive roughness study resulted in a swept ramp configuration, scaled to be roughly 0.6 of the calculated boundary layer thickness, being selected for the Mach 7 flight vehicle. For the active blowing study, the manifold pressure was systematically varied (while monitoring the mass flow) for each configuration to determine the jet penetration height, with schlieren, and transition movement, with the phosphor system, for comparison to the passive results. All the blowing concepts tested, which included various rows of sonic orifices (holes), two- and three-dimensional slots, and random porosity, provided transition onset near the trip location with manifold stagnation pressures on the order of 40 times the model surface static pressure, which is adequate to ensure sonic jets. The present results indicate that the jet penetration height for blowing was roughly half the height required with passive roughness elements for an equivalent amount of transition movement.

Berry, Scott A.↗

Interplanetary Microlaser Transponders

The feasibility of an asynchronous (i.e. independently firing) interplanetary laser transponder, capable of ranging between Earth and Mars and using the automated SLR2000 Satellite Laser Ranging (SLR) system as an Earth base station, has been suggested. Since that time, we have received a small amount of discretionary funding to further explore the transponder concept and to develop and test an engineering breadboard. Candidate operational scenarios for acquiring and tracking the opposite laser terminal over interplanetary distances have been developed, and breadboard engineering parameters were chosen to reflect the requirements of an Earth-Mars link Laboratory tests have been devised to simulate the Earth- Mars link between two independent SLR2000 transceivers and to demonstrate the transfer of range and time in single photon mode. The present paper reviews the concept of the asynchronous microlaser transponder, the transponder breadboard design, an operational scenario recently developed for an asteroid rendezvous, and the laboratory test setup. The optical head of the transponder breadboard fits within a cylinder roughly 15 cm in diameter and 32 cm in length and is mounted in a commercial two axis gimbal driven by two computer-controlled stepper motors which allows the receiver optical axis to be centered on a simulated Earth image. The optical head is built around a small optical bench which supports a 14.7 cm diameter refractive telescope, a prototype 2 kHz SLR2000 microlaser transmitter, a quadrant microchannel plate photomultiplier (MCP/PMT), a CCD array camera, spatial and spectral filters, assorted lenses and mirrors, and protective covers and sun shields. The microlaser is end-pumped by a fiber-coupled diode laser array. An annular mirror is employed as a passive transmit/receive (T/R) switch in an aperture-sharing arrangement wherein the transmitted beam passes through the central hole and illuminates only the central 2.5 cm of the common telescope (adequate to achieve a 10 arcsecond full laser beam divergence) while the receiver uses the remainder of the 14.7 cm aperture. Additional electronic instrumentation includes the diode pump array and associated heat sink and current drivers, rubidium frequency standard, timing distribution module, range gate generator, a recently developed all-digital correlation range receiver, and system computer. Acquisition of the opposite transponder terminal requires a search within a three-dimensional volume determined by the initial pointing uncertainty and a maximum 500 microsecond uncertainty in the laser time of fire at the opposite terminal for totally uncorrelated Earth and spacecraft clocks. The angular search is aided by a sensitive CCD array capable of imaging the Earth, Moon, and surrounding stars within the nominal + 0.5 degree cone of uncertainty associated with the initial pointing of a spacecraft body or microwave communications dish.

Degnan, John J.↗

Development and Integration of a Stochastic Clad Damage Propagation Model into PRONGHORN-SC Subchannel Analysis Code

The failure of fuel pins in nuclear reactors is intrinsically stochastic. Typically, a combination of variation in manufacturing that affects the material characteristics and the fuel assembly dimensions, variation in operating conditions, such as local power, coolant flow rate, and irradiation induced changes in material properties lead to a large uncertainty in failure margin of the fuel pins. Failure, therefore, may occur in exceptional pins with adverse combinations of these variations. Upon a metal fuel pin (U-Pu-Zr/HT9) failure, depressurization of the fuel pin takes place by release of fission gas, liquid sodium bond, and potentially solid fuel particles or molten/eutectic fuel droplets through the hole in cladding. The effect of a fission gas jet on neighbor fuel pins and possible propagation of a clad damage during normal operation was studied experimentally in 1970s and it was found that the post-failure fission gas jet insulates the jet impingement area of the target fuel pin surface and could increase the target pin’s surface temperature by as much as 100 – 200 K during the failed pin depressurization. It was concluded that the effect should not lead to fuel pin failure propagation during normal operation. In accident scenarios of sodium and lead fast reactors such as Unprotected Loss-Of-Flow (ULOF) or Unprotected Transient Over Power (UTOP), the fuel pins can be subjected to higher clad temperatures and fuel pin pressures or fuel clad mechanical/chemical interaction where thermal creep margin becomes significantly lower compared to the normal operation conditions. Therefore, possible stochastic failure and the post-failure fission gas/fuel jet impingement could be critical in order to predict fuel pin failure propagation. Pin depressurization due to fission gas release may degrade the heat transfer by formation of a gas blanket on a neighboring pin surface, which is a local phenomenon, and by causing coolant flow deceleration and starvation, which could affect a surrounding region as well. Furthermore, the potential presence of solid fuel particles or molten fuel at the time of clad failure could boost post-failure jet induced degradation even further. The present study models the U-Pu-Zr/HT9 metal fuel pin failure and stochastic clad damage propagation by biased sampling based on a Cumulative Damage Fraction (CDF) type clad failure criterion and the normal distribution of fuel failure probability density as a function of logarithm of Cumulative Damage Fraction. In addition, the effect of post-failure fission gas jet on heat transfer degradation is modeled for the target pins. This model is called stochastic Clad Damage Propagation (CDAP). The CDAP model is now fully integrated into developmental version of PRONGHORN-SC subchannel analysis code, allowing for modeling local failures and its propagation potential. Section 2 describes the components of the CDAP models. Section 3 describes the model implementation to PRONGHORN-SC and input specifications. Section 4 describes the CDAP model validation coupled to PRONGHORN-SC.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Satellite Mapping of the Earth's Ozone and Sulfur Dioxide

The Total Ozone Mapping Spectrometer (TOMS) instruments are spatially-scanning UV spectrometers that have produced daily global images of total ozone over the last 21 years since the launch of the Nimbus 7 satellite. The instruments use a total ozone retrieval algorithm pioneered by J.V. Dave and C. L. Mateer for the Nimbus 4 Backscatter Ultraviolet (BUV) instrument, designed by D.F. Heath. The TOMS ozone maps have revealed the relations between total ozone and atmospheric dynamics, and shown the dramatic losses of ozone in the Antarctic ozone hole and the Northern hemisphere. The accepted long-term trends in global, regional, and local ozone are derived from data from the Nimbus 7 TOMS and three successive TOMS flights on Russian, Japanese, and American satellites. The next TOMS flight will be launched in 2000. The contiguous mapping design and fortuitous choice of TOMS wavelengths bands also permitted imaging of a second atmospheric gas, sulfur dioxide, which is transient due to its short lifetime. The importance of this measurement was first realized after the eruption of El Chichon volcano in 1982. The extreme range of sizes of volcanic eruptions and the 'associated danger require observations from a distant observing platform. The first quantitative time series of the input of sulfur dioxide by explosive volcanic eruptions into the atmosphere thus was developed from the TOMS missions. Finally, the Rayleigh and aerosol scattering spectral characteristic and reflectivity complete the four dominant pieces of information in the near UV albedo of the Earth. The four parameters are derived with a linear algorithm, the absorption coefficients of the gases, and effective paths computed from radiative transfer tables. Absorbing aerosol clouds (smoke, dust, volcanic ash) are readily identified by their deviation from a Rayleigh signature. The greatest shortcoming of the TOMS dataset is the 24 hour time resolution that is produced by the polar orbit of the satellite. Dynamic phenomena, such as upper air fronts that modulate total ozone and volcanic eruptions of sulfur dioxide and ash, cannot be adequately resolved. It is hoped that UV observations from geostationary satellites will soon be made to test the value of this unique information in weather forecasting and aviation safety.

Krueger, Arlin↗

Satellite Mapping of the Earth's Ozone and Sulfur Dioxide

The Total Ozone Mapping Spectrometer (TOMS) instruments are spatially-scanning UV spectrometers that have produced daily global images of total ozone over the last 21 years since the launch of the Nimbus 7 satellite. The instruments use a total ozone retrieval algorithm pioneered by J.V. Dave and C. L. Mateer for the Nimbus 4 Backscatter Ultraviolet (BUV) instrument, designed by D.F. Heath. The TOMS ozone maps have revealed the relations between total ozone and atmospheric dynamics, and shown the dramatic losses of ozone in the Antarctic ozone hole and the Northern hemisphere. The accepted long-term trends in global, regional, and local ozone are derived from data from the Nimbus 7 TOMS and three successive TOMS flights on Russian, Japanese, and American satellites. The next TOMS flight will be launched in 2000. The contiguous mapping design and fortuitous choice of TOMS wavelengths bands also permitted imaging of a second atmospheric gas, sulfur dioxide, which is transient due to its short lifetime. The importance of this measurement was first realized after the eruption of El Chichon volcano in 1982. The extreme range of sizes of volcanic eruptions and the associated danger require observations from a distant observing platform. The first quantitative time series of the input of sulfur dioxide by explosive volcanic eruptions into the atmosphere thus was developed from the TOMS missions. Finally, the Rayleigh and aerosol scattering spectral characteristic and reflectivity complete the four dominant pieces of information in the near UV albedo of the Earth. The four parameters are derived with a linear algorithm, the absorption coefficients of the gases, and effective paths computed from radiative transfer tables. Absorbing aerosol clouds (smoke, dust, volcanic ash) are readily identified by their deviation from a Rayleigh signature. The greatest shortcoming of the TOMS dataset is the 24 hour time resolution that is produced by the polar orbit of the satellite. Dynamic phenomena, such as upper air fronts that modulate total ozone and volcanic eruptions of sulfur dioxide and ash, cannot be adequately resolved. It is hoped that UV observations from geostationary satellites will soon be made to test the value of this unique information in weather forecasting and aviation safety.

Krueger, Arlin↗

Quantitative relationships between film morphology, charge carrier dynamics, and photovoltaic performance in bulk-heterojunction binary vs. ternary acceptor blends

Addressing pertinent and perplexing questions regarding why nonfullerene acceptors (NFAs) promote higher power conversion efficiencies (PCEs) than traditional fullerenes and how photoactive bulk heterojunction (BHJ) film morphology, charge photogeneration, and recombination dynamics dictate solar cell performance have stimulated many studies of polymer solar cells (PSCs), yet quantitative relationships remain limited. Better understanding in these areas offers the potential to advance materials design and device engineering, afford higher PCEs, and ultimate commercialization. Here we probe quantitative relationships between BHJ film morphology, charge carrier dynamics, and photovoltaic performance in model binary and ternary blend systems having a wide bandgap donor polymer, a fullerene, and a promising NFA. We show that optimal PC 71 BM incorporation in a PBDB-TF:ITIC-Th binary system matrix retains the original π-face-on orientation, ITIC-Th crystallinity and BHJ film crystallite dimensions, and reduces film upper surface ITIC-Th segregation. Such morphology changes together simultaneously increase hole (μ h ) and electron (μ e ) mobilities, facilitate light-activated ITIC-Th to PC 71 BM domain electron delocalization, reduce free charge carrier (FC) bimolecular recombination (BR) within PBDB-TF:ITIC-Th mixed regions, and increase FC extraction pathways viaPBDB-TF:PC 71 BM pairs. The interplay of these effects yields significantly enhanced inverted cell short-circuit current density (J SC ), fill factor (FF), and PCE. Unexpectedly, we also find that excessive PC 71 BM in the PBDB-TF:ITIC-Th binary system alters the PBDB-TF orientation to π-edge-on, increases large scale PC 71 BM-rich aggregations and BHJ upper surface PC 71 BM composition. Further, these morphology changes increase parasitic decay processes such as intersystem crossing from photoexcited PC 71 BM, compromising the J SC , FF, and PCE metrics. ITIC-Th X-ray diffraction reveals a unique sidechain-dominated molecular network with previously unknown sidechain-end group stacking, rationalizing the STEM and GIWAXS results, photophysics, and the high μ e . DFT computation reveals charge transfer networks within ITIC-Th crystallites, supporting excited-state electron delocalization from ITIC-Th to PC 71 BM. This structure–property understanding leads to a newly reported NFA blend with PCE near 17%.

14 SOLAR ENERGY↗